Cain, who was arrested two days later, already faced charges of attempted murder, armed robbery and kidnapping in the shooting that nearly killed 25-year-old good Samaritan Peter Gold.

Euric Cain, 21, was charged Wednesday in a rape and carjacking the day after a shooting that left a Tulane University medical student nearly dead, police said. (New Orleans Police Department)

Investigators believe Cain shot him in the stomach and would have shot him in the head if his gun didn't jam. Police said Gold sprang into action to protect a woman Cain was dragging toward a car around 4 a.m. in the Lower Garden District Nov. 20. A graphic security camera video of the sequence drew national attention.

Now Cain - whose 17-year-old girlfriend Nictoria Washington is accused of sheltering him after the Nov. 20 shooting - has first-degree rape, second-degree kidnapping, armed robbery and carjacking charges on his rap sheet, according to NOPD. He's also considered a top suspect in a series of rapes and sexual assaults reported in October and November, the Times-Picayune reported.

"He is, in our opinion, a very dangerous individual," NOPD Superintendent Michael Harrison said at a news conference Wednesday. "And that's why we're working so hard to present a very good, solid case on the rape and the shooting of Peter Gold, to make sure he's put away for a very long time, exactly where he belongs."

Police said Cain shot a good Samaritan who broke up his kidnapping attempt on a woman in the Lower Garden District and would have killed him if his gun didn't jam. (NOPD Sixth District via YouTube)

Police said Cain put a gun to the couple's heads and demanded they fork over their cash and credit cards after he got into the vehicle at St. Philip and Henriette Delille streets in the Treme neighborhood. He then commanded the woman to drive to an abandoned school parking lot about four miles away in the Desire area, according to cops.

Cain's girlfriend Nictoria Washington, 17, is accused of harboring Cain when he became the target of a massive manhunt following the Nov. 20 shooting. (Orleans Parish Sheriff’s Office)

He sexually assaulted the couple in the back seat and then told them he would kill them if they alerted police, according to arresting documents cited by WVUE-TV.

Detectives later found their Ford Focus in Cain's possession when he was cuffed and linked him to DNA evidence recovered from the car, the documents said. Investigators also traced a credit card purchase with one of the victims' cards to a store where surveillance footage showed Cain using the card.

Authorities have raised Cain's bond to $7 million from its earlier $6 million total due to the new charges. Detectives are looking into the earlier crime spree to see if his DNA matches samples taken from the other scene, Harrison said Wednesday.

A still image from WVUE shows the abandoned school parking lot near Abundance and Press streets where police said Cain raped a woman and forced a man to perform oral sex on him at gunpoint. (WVUE)

"Right now, we know of these two," Harrison said. "But we're doing our due diligence to make sure that he's not connected to any other crimes. And if he is, he's going to be arrested and prosecuted for those crimes as well."